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Danny's First Paper!

Danny's First Paper!

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Published by Danny Taller
My first paper published in Physical Review Letters.
My first paper published in Physical Review Letters.

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Published by: Danny Taller on Dec 03, 2012
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12/04/2012

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Self-Similar Micron-Size and Nanosize Drops of Liquid Generated by Surface Acoustic Waves
Daniel Taller,
1
David B. Go,
1
and Hsueh-Chia Chang
2,
*
1
 Department of Aerospace and Mechanical Engineering, University of Notre Dame, Notre Dame, Indiana 46556, USA
2
 Department of Chemical and Biomolecular Engineering, Center for Microfluidics & Medical Diagnostics,University of Notre Dame, Notre Dame, Indiana 46556, USA
(Received 13 September 2012; published 27 November 2012)A planar surface acoustic wave on a solid substrate and its radiated sound into a static liquid dropproduce time-averaged, exponentially decaying acoustic and electric Maxwell pressures near the contactline. These localized contact-line pressures are shown to generate two sequences of hemispherical satellitedroplets at the tens of microns and submicron scales, both obeying self-similar exponential scaling butwith distinct exponents that correspond to viscous dissipation and field leakage length scales, respectively.The acoustic pressure becomes dominant when the film thickness exceeds (
1
=
4
 
) of the surface acousticwave wavelength and it affects the shape and stability of the mother drop. The Maxwell pressure of thenanodrops, which exceeds ten atmospheres, is sensitive to the contact angle.
DOI:10.1103/PhysRevLett.109.224301PACS numbers: 43.35.Pt, 68.35.Iv, 78.67.Tf 
Surface acoustic waves (SAWs) are elastic compressionsurface waves generated on piezoelectric crystals by alter-nating current (ac) electric fields sustained by an interdi-gitated electrode transducer [13]. Both compression and electric traveling waves of specific wavelength can begenerated on the surface of the crystal. Like plasmonicoptical surface waves, SAWs are dispersive [4], but unlikeoptical waves, theyarehighlynonlinear[5].Surfaceacous-tic compression waves involve nanometer high deforma-tiononthesolidandhavein-phase[6]electriccomponents.Historically, SAW devices have found widespread useas filters, oscillators, and transformers in the electronicsindustry [2]. More recently, they have been incorporatedinto microfluidic devices, where they can be used to mani-pulate fluids on the surface of the SAW device or dispersefluid into aerosols, with applications ranging from massspectrometry [68] to pulmonary drug delivery [9,10]. Extensive studies have been undertaken to characterizebreakup of liquid drops by SAWs [11,12] to generate jets [13,14] and aerosols [15,16]. Microfluidic and mass spectrometry applications areparticularly intriguing, as they involve the scattering of the surface wave into a drop or film on the substrate.This scattering is like optical refraction, but the wedge-shaped geometry of the drop at the scattering location(contact line) suggests an electric hot spot similar to aplasmonic hot spots or singular scattering near the tip of a wedge [17,18]. Since the SAW wavelength (
SAW
%
132
m
) is much larger than the scattering region, an‘electrostatic’’ approximation is permissible for the acous-tic wave equation to yield a quasistatic analysis of theacoustic field near the contact line, as is commonly donefor the Maxwell wave equation for optics [6,17]. It is indeed known that the acoustic waves that scatterinto a bulk drop or a liquid film will generate high acousticpressure at the contact line [19]. This acoustic radiationpressure can drive a dc streaming flow that is suspectedto be responsible for a contact line instability that pulls athin film of liquid away from the bulk and causes rupture[20]. However, the time-averaged system can also remainat equilibrium, and the acoustic pressure can be com-pensated by capillary pressure resulting in a quasistaticequilibrium [20].While the scattered sound waves produce an acousticpressure in the bulk liquid, the traveling electric field of the transmitted SAW on the piezoelectric substrate canproduce dielectric polarization at the solid-liquid interfacewith a corresponding electric Maxwell pressure. The sin-gularLaplaceharmonicsat geometricsingularities[2125] also suggest that the electric traveling wave will gene-rate an electric field maximum (or singularity) near thecontact line, which could be responsible for the ionizationobserved in SAW mass spectrometry. It follows that theSAW-induced Maxwell pressure can also balance the cap-illary pressure to generate similar small satellite dropletsat the contact line or even quasistatic cones, albeit at ashorter length scale since the Maxwell pressure is expectedto be shorter range than the acoustic pressure. This balanceof electric and capillary pressures at the contact line isanalogous to dc Taylor and ac electrospray cones, wherean electric Maxwell pressure is balanced by the capillarypressure so that both vary toward infinity in the samemanner approaching the cone tip [22,25]. In fact, previous experimental and numerical studies of SAWs alongwedge-shaped channels show both high acoustic and electric fieldsat the tip of the wedge [26,27]. In the present Letter, we experimentally confirm thepresence of these effects for the first time and offer scalingtheories to clarify where the acoustic and Maxwell pres-sures dominate. For the quasistatic structures to exist, it isimportant that the drop does not move under the influenceof the SAW. As such, we generate pinned stationary dropsPRL
109,
224301 (2012)PHYSICAL REVIEW LETTERS
week ending30 NOVEMBER 2012
0031-9007
=
12
=
109(22)
=
224301(5) 224301-1
Ó
2012 American Physical Society
 
by extracting small amounts (
$
0
:
1
L
) of liquid ontoa SAW device via a paper wick such that the drop isconstrained by contact with the paper.The SAW device for the present study was fabricatedusing standard photolithographic methods on a 127.68
yx
-cut lithium niobate (
LiNbO
3
) substrate. The SAW de-vice was fabricated with focusing electrodes as pioneeredby Wu
et al.
[28] and used in previous studies of SAW formass spectrometry and microfluidics [6,7]. A small plastic weigh boat was used as a reservoir to supply the workingfluid, deionized (DI) water. Cleanroom paper (TX 609TechniCloth Non Woven Wipers) was used to wick theworking fluid onto the substrate so that fluid could besupplied continuously. For all experiments, an ac voltagewas applied to the SAW transducers via a waveform gen-erator (Agilent 33250A) attached to an amplifier (E&I325LA) at a frequency of 
SAW
¼
29
:
5 MHz
. Prior tooperation, the paper wick was saturated with fluid fromthe reservoir and brought to the edge of the SAW device.Upontheapplicationofacpower,SAWsweregeneratedandliquid was drawn from the saturated paper onto the devicesurface, andatsufficient power aerosolized.Thiswasfilmedusing a high-speed camera (Photron Fastcam SA4) with aNavitar telescopic lens (
$
48
Â
magnification) adjacent tothe SAW device. A schematic of the SAW device and place-ment of the paper wick is shown in Fig.1(a).At low powers, prior to the onset of aerosolization, aliquid film was extracted from the paper by SAWs and asequence of self-similar satellite droplets formed on thesubstrate, as discussed above and shown in Fig.1(a). Thesubstrate was either cleaned with acetone or was treatedwith trichloro(1H,1H,2H,2H-perfluorooctyl)silanevia evap-oration to change the liquid contact angle. The dropletsincrease in radius closer to the paper wick, which is alongthe direction of SAW propagation (
 x
coordinate), and thesequence of droplet sizes has a strong dependence on thecontact angle [Fig.2(b)].We model the droplet size distribution as a train of hemispherical droplets whose radii are controlled by theacoustic or Maxwell pressure that decays into the liquid.The
n
th hemisphere thus has radius
R
n
, with position
L
n
¼
2
P
nm
¼
1
R
m
, so that the smallest droplet of radius
R
1
beginsat
L
0
¼
0
, the next droplet begins at
L
1
¼
2
R
1
, and so on.Assuming that the droplet radius
R
n
is governed by theapplied pressure at
L
n
À
1
, given by
P
SAW
ð
L
n
À
1
Þ
, a balanceof capillary pressure and the acoustic or Maxwell pressurerequires that
2
=R
n
¼
P
SAW
ð
L
n
À
1
Þ
, where
is surfacetension. Hence,
L
n
¼
4
X
nm
¼
1
1
P
SAW
ð
L
m
À
1
Þ
:
(1)In the case that acoustic pressure is dominant,
P
SAW
isdue to viscous dissipation of a bulk acoustic wave thatrefracts off the substrate at an angle corresponding to theRayleigh scattering angle when the SAW enters into theliquid. The leading-order theory for the propagation andviscous attenuation of the sound wave produces a fluiddisplacement velocity
u
1
with zero time average.However, the time averaged Bernoulli dynamic pressure,
h
u
21
=
2
i
, where
is the ambient equilibrium density, isnonzero and produces a time-averaged acoustic radiationpressure [9,19],
P
acoustic
¼
12
ð
1
þ
2
Þ
 A
2
!
2
e
À
2
ð
k
 x
 x
þ
k
y
y
Þ
 ;
(2)which decays exponentially into the fluid in the samedirectionofpropagationas thevelocity
u
1
withacharacter-istic decay length of 
l
R
¼
1
=
2
k
R
. The Rayleigh acousticdecay constant
k
R
is in the direction of the Rayleigh refrac-tion angle
R
from the normal, as shown in Fig.1(a), andhas components
k
 x
¼
k
R
sin
ð
R
Þ
and
k
y
¼
k
R
cos
ð
R
Þ
,where the Rayleigh angle is
R
¼
sin
À
1
ð
w
=V 
R
Þ
usingSnell’s law for the refracted liquid sound wave velocity
w
andtheSAWRayleighwavevelocity
R
.Theparameter
!
¼
2
f 
SAW
is the angular frequency,
A
is the amplitudeof the SAW, and
2
¼
cot
2
ð
R
Þ ¼ ð
R
=V 
w
Þ
2
À
1
is anattenuation constant arising from the change in speed of the wave from the solid to the liquid phase.The radiation pressure (2) can sometimes drive a stream-ing flow and is hence referred to as a streaming pressure.However, for a thin film, it can be balanced quasistatically
FIG. 1 (color online). (a) Schematic of SAW device producinga droplet train from a pinned liquid film (side view) with insetshowing an experimental image of the droplet train using DIwater. The acoustic waves refract into the fluid at Rayleigh angle
R
. (b) Top view of surface droplets for contact angles 45
(left)and 80
(right). Note that the Maxwell droplets decay muchmore quickly in the image on the right due to the change incontact angle.
PRL
109,
224301 (2012)PHYSICAL REVIEW LETTERS
week ending30 NOVEMBER 2012
224301-2
 
by an interfacial capillary pressure and a pressure fieldwithin the film without generating a dc flow. This radiationpressure is derived for an infinitely large drop. Our originaldrop size is that of the extracted film with a thickness of about one millimeter and is indeed much larger than theSAW wavelength. As a simple model, we assume theacoustic radiation pressure of the original film remainsvalid as the film thins near the contact line and dropletssmaller than the SAW wavelength are formed. Since thethin film that breaks up into droplets is slender in aspectratio, we also neglect the decay of the acoustic radiationpressure in the vertical direction and use the averageacoustic pressure at a particular droplet to estimate itscapillary pressure and diameter.Combining Eqs. (1) and (2) with these approximations, we obtain
L
n
þ
1
¼
L
n
þ
8
ð
1
þ
2
Þ
 A
2
!
2
e
2
k
 x
L
n
 ;
(3)such that the radius of the droplets away from the pinnedfilm will decrease exponentially away from the pinned filmwith a characteristic decay length that is half of theRayleigh decay length. If we transpose Eq. (3) so that thedifference of the lengths
L
n
þ
1
and
L
n
is the droplet diame-ter
D
, and
L
n
is equivalent to position
x
, then the scalingrelationship for droplet size becomes
ln
ð
D
Þ /
x
with con-stant of proportionality
2
k
 x
. Figure2(a)shows experimen-tal data using DI water as the working fluid at a variety of SAW powers and confirms this exponential relationshipwith
x
taken to be zero where the smallest visible dropletsare seen (more details on this measurement included in theSupplemental Material [29]). Further, when the SAW am-plitude is scaled away, the different data sets all collapseaccording to the scaling suggested in Eq. (3), as shown inFig.2(b). The distance
L
transition
, from where the smallestvisible droplets are seen to the transition region wherethe decay rate changes, is measured experimentally. Thedecay length
l
 x
and the drop diameter at the transitionregion
D
transition
are adjusted empirically but both will becompared to predicted values from our theory for theMaxwell drops.Curiously, there are actually two sets of collapsed datawith two distinct exponents in Fig.2.For the larger drop- lets (at greater
x
), an acoustic decay constant
k
 x
value of 
6800 m
À
1
(corresponding to
l
 xR
¼
1
=k
 x
¼
147
m
) canbe extracted and it is on the same order of magnitude,though larger than the reported value for water of 
1370 m
À
1
or
l
 xR
¼
730
m
[19]. We attribute this discrep-ancy to droplets coalescing prior to measurement, whichoccurs most dramatically for larger droplets, thus artifi-cially increasing the slope. We estimate the acoustic pres-sure by assuming an amplitude
A
on the order of tennanometers, consistent with past studies [30], and find
P
acoustic
$
10
2
10
3
Pa
provides sufficient pressure to sus-tain droplets with diameter
D
on the order of tens tohundreds of microns, corresponding to the larger droplets.Thus it is clear that the larger sequence of satellite dropletsare generated because of the acoustic pressure near thecontact line, and the sequence of these acoustic Rayleighdrops is due to a static balance between the exponentiallydecaying acoustic pressure and the local capillary pressure.The second set of collapsed data for the sequence of smaller droplets suggests that a different exponentiallydecaying pressure with a different decay rate must be atplay closer to the original contact line. We attribute thissequence of satellite drops to the Maxwell pressure due tothe electric field of the transmitted SAWs that remain onthe substrate. Because of the finite wavelength
SAW
of theSAW, its electric field decays in the direction normal to thesurface due to field leakage both out into the gas phase and
FIG. 2 (color online). (a) Plot of 
ln
ð
D
Þ
as a function of 
x
for data acquired at different SAW powers along with linear curve fits.All units are in meters and
c
¼
45
for the untreated substrate. The slopes of the linear fits are equivalent to the decay constant.(b) The data sets collapsed on a single plot, where
D
transition
is the droplet size where the transition for the two droplet families occurs(
%
11
m
),
L
transition
is the measured
x
location of the transition, and
l
 x
is the decay length of the Maxwell pressure. Two sets of data(open and closed symbols) were acquired for each power setting.
PRL
109,
224301 (2012)PHYSICAL REVIEW LETTERS
week ending30 NOVEMBER 2012
224301-3

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